期刊
NANO LETTERS
卷 20, 期 2, 页码 1252-1261出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.9b04719
关键词
Single-atom catalysts; lithium-sulfur batteries; catalytic conversion; graphene; density functional theory simulation
类别
资金
- Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the U.S. Department of Energy, under the Battery Materials Research program
- Battery 500 Consortium program
- Natural Key Research and Development Program of China [2019YFA0705703]
- National Natural Science Foundation of China [51872293, 11404017]
- Beijing Natural Science Foundation [2192029]
- Technology Foundation for Selected Overseas Chinese Scholar
- Ministry of Human Resources and Social Security of China
- program for New Century Excellent Talents in University [NCET-12-0033]
- Australian Research Council [DP150102044, DP180100731, DP180100568]
- U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering Division
Lithium-sulfur (Li-S) batteries are promising next-generation energy storage technologies due to their high theoretical energy density, environmental friendliness, and low cost. However, low conductivity of sulfur species, dissolution of polysulfides, poor conversion from sulfur reduction, and lithium sulfide (Li2S) oxidation reactions during discharge-charge processes hinder their practical applications. Herein, under the guidance of density functional theory calculations, we have successfully synthesized large-scale single atom vanadium catalysts seeded on graphene to achieve high sulfur content (80 wt % sulfur), fast kinetic (a capacity of 645 mAh g(-1) at 3 C rate), and long-life Li-S batteries. Both forward (sulfur reduction) and reverse reactions (Li2S oxidation) are significantly improved by the single atom catalysts. This finding is confirmed by experimental results and consistent with theoretical calculations. The ability of single metal atoms to effectively trap the dissolved lithium polysulfides (LiPSs) and catalytically convert the LiPSs/Li2S during cycling significantly improved sulfur utilization, rate capability, and cycling life. Our work demonstrates an efficient design pathway for single atom catalysts and provides solutions for the development of high energy/power density Li-S batteries.
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